THE DECADE OF DEPLETED URANIUM ASAF DURAKOVIC M.D., D.V.M., MSc, - PowerPoint PPT Presentation

THE DECADE OF DEPLETED URANIUM

ASAF DURAKOVIC M.D., D.V.M., MSc, Ph.D., F.A.C.P. Professor of Medicine, Radiology and Nuclear Medicine URANIUM MEDICAL RESEARCH CENTRE Washington, DC, USA Richmond Hill, Ontario, Canada

An Update of the Quantitative Analysis of Uranium Isotopes in British, Canadian, and United States Gulf War Veterans

A. Durakovic, P. Horan, L. Dietz - Uranium Medical Research Centre Washington, DC, USA Richmond Hill, Ontario, Canada Department of Earth Sciences Memorial University of Newfoundland St. Johns, Newfoundland, Canada

The Objective of the Study To determine the quantities and ratios of uranium isotopes in the urine and organs of the Gulf War Veterans exposed to depleted uranium (DU) by the inhalational route of internal contamination .

Patients, Materials, and Methods Twenty-Seven British, Canadian, and United States veterans presenting with complex non-specific clinical symptomatology of the Gulf War Illness had their 24hrs urine samples quantitatively determined for 234 U, 235 U, 236 U, and 238 U by the method of mass spectometric analysis at Atlantic Universities Radiogenic Isotope Facility. St. Johns, Newfoundland, Canada

Radiochemical Analysis • The urine samples were collected and transported under controlled circumstances in sealed plastic vials, weighed into savillex-teflon screw-cap jars (15ml) and evaporated to dryness at 80-100 degrees C. • All samples were repeatedly evaporated three times after the addition of 4ml of double distilled concentrated nitric acid.

• Each sample was separated into an isotopic concentration and isotopic dilution fraction, by adding 3.1N hydrochloric acid to each sample. • Half of each sample was transferred to the savillex-teflon jar (7ml) & accurately weighed.

Mass Spectrometry • Uranium was separated and collected in both fractions after ion exchange preparation with DOWEX analytical grade AGL-X8 ion exchange resins with a modified HBr technique.

• The isotopic composition was measured by a multi-collector Finnigan mass spectrometer using secondary electron multiplier (SEM) detector and ion counting system. • The uranium blank control has been determined to by 0.45 picograms and 960U standard, measured by the same procedure.

Humans ingest or breathe in uranium. Sources are: 1) Drinking water which is filtered through the ground 2) Eating vegetables grown in our gardens 3) Breathing in dust and dirt on windy days Hypothetical measurement of urine specimen: 238 U/ 235 U = ~137.88 Every person will have trace amounts of naturally occurring uranium in their system. We absorb it through the vegetable we eat and through the water we drink which is filtered through the soil and rocks that we live. We can also get small amounts by inhaling or ingesting dirt and dust blowing around in the breeze. So if I measured someone’s urine specimen from my family, I would see this naturally occurring 238 U/ 235 U ratio of approximately 137.88.

Atlantic Universities Radiogenic Isotope Facility (AURIF) The Atlantic Universities Radiogenic Isotope Facility (AURIF) was created in 1989 to analyze geological samples for radiogenic isotopic tracers studies. Since its inception, AURIF has analysed samples for numerous scientists worldwide. The combined research experience of the scientific personnel in AURIF in dealing with the U/Pb isotopic system spans over 30 years with more than 5000 U/Pb analyses completed. Data from this lab has been published in peer- reviewed journals for more than 9 years.

Depleted Uranium : DU for short “left-over” product during the enrichment process for nuclear fuel rods or nuclear weapons. DU shrapnel measured in AURIF lab 238 U = 99.7945%, 235 U = 0.2026%, 234 U = 0.0012%. Key ratio of interest: 238 U/ 235 U = 491.87 ± 0.16 (2σ absolute) The nuclear industry refines mined U 3 O 8 and removes the majority of 235 U and 234 U for use in nuclear fuel rods. This enrichment process creates a “left over” form of uranium with substantially less 235 U and increased 238 U abundance as seen in this slide. This “left over” uranium is referred to as depleted uranium. The 238 U/ 235 U ratio measured from one particular piece of shrapnel is 491.87 ± 0.16 (2 σ ). I already mentioned one use of DU as ballast in airplanes manufactured before the mid –1980’s. Another use of DU has been in shell casing for military armaments. The shells are very hard and will easily pierce armour. Upon impact, the DU in the shell casing ignites and burns causing massive damage.

AURIF uses a Finnigan MAT 262V solid source thermal ionization mass spectrometer with 8 faraday detectors and one secondary electron multiplier – ion-counting system.

The sample, when loaded, is ionized by passing a current through the filament with the dried sample on it. To ensure that the each ion (isotopic mass) is centred in each detector, the beam of ions is focused using a series of lenses located just aft of the source.

The mass spectrometer has a large electromagnet that facilitates the separation of charged particles or ions.

Illustration of mass separation with the Finnigan electromagnet Courtesy of Finnigan MAT As the beam of ions pass out through the “line of sight” or beam valve, it encounters a strong magnetic field created by the large electromagnet. Since the beam contains ions of different masses, it splits into individual beams, one per isotopic mass present in the sample. So for uranium, one beam enters the magnetic field and produces individual 238 U, 235 U and 234 U (and even sometimes 236 U if present in the sample).

Table 1: Quantitative Data for Individual Samples No. Patient U 238 U 235 U238/U235 Sigma 1 G.B. 99.2782 0.7145 139.0 1.3 2 B.B 99.2742 0.7076 140.3 0.2 3 R.B. 99.2782 0.7145 139.0 1.3 4 L.B. 99.2738 0.7180 138.3 0.5 5 D.B. 99.2701 0.7233 137.5 0.5 6 P.C. 99.2570 0.7210 137.7 0.5 7 C.C. 99.2738 0.7113 139.6 0.4 8 R.G.D. 99.3154 0.6758 147.0 0.7 9 J.G. 99.7565 0.2339 426.6 3.7 10 W.H. - - - - - - - - - - - - 11 J.H. - - - - - - 153.0 0.1 12 M.K. 99.2762 0.7152 138.8 0.8 13 C.P.L. 99.2702 0.7200 137.9 0.5 14 G.L. - - - - - - - - - - - - 15 K.I.M. 99.4280 0.5663 175.6 1.7 16 T.N. 99.2963 0.6925 143.4 3.4 17 C.O. 99.2811 0.7135 139.1 0.9 18 A.P. 99.3456 0.6495 153.0 0.3 19 T.R. 99.5564 0.4346 229.1 1.3 20 P.R. 99.2742 0.7189 138.1 0.8 21 S.R. 99.5603 0.4304 231.3 1.6 22 F.S. (A) 99.4876 0.4945 201.2 5.9 23 F.S. (B) 99.2693 0.7189 138.1 1.7 24 V.S. 99.7113 0.2830 352.4 1.5 25 M.D.T - - - - - - - - - - - - 26 R.W. 99.3025 0.6825 145.5 1.4 27 A.W. 99.3862 0.4966 200.1 1.2

Table 2: Summary of Quantitative Data for Individual Samples U 238 U 235 U238/U235 Sigma Negative 99.2726 0.7166 138.6 0.8 Std. Dev. 0.00625 0.0046 0.862 Std. Error 0.00188 0.0014 0.260 Positive 99.4561 0.5248 208.4 1.42 Std. Dev. 0.1598 0.1575 87.51 Std. Error 0.0461 0.0455 24.27 Totals 99.3683 0.6165 176.4 1.18 Std. Dev. 0.1469 0.1483 72.51 Std. Error 0.0306 0.0309 14.80 P-Value 0.00108 0.00072 0.00696

Table 3: Quantitative Data for Positive Samples No. Patient U 238 U 235 U238/U235 Sigma 3 R.B. 99.2782 0.7145 139.0 1.3 8 R.G.D. 99.3154 0.6758 147.0 0.7 9 J.G. 99.7565 0.2339 426.6 3.7 11 J.H. - - - - - - 153.0 0.1 15 K.I.M. 99.4280 0.5663 175.6 1.7 16 T.N. 99.2963 0.6925 143.4 3.4 18 A.P. 99.3456 0.6495 153.0 0.3 19 T.R. 99.5564 0.4346 229.1 1.3 21 S.R. 99.5603 0.4304 231.3 1.6 22 F.S. (A) 99.4876 0.4945 201.2 5.9 24 V.S. 99.7113 0.2830 352.4 1.5 26 R.W. 99.3025 0.6825 145.5 1.4 27 A.W. 99.3862 0.4966 200.1 1.2 Totals 99.4561 0.5248 208.4 1.42 Std. Dev. 0.1598 0.1575 87.51 Std. Error 0.0461 0.0455 24.27

Table 4: Quantitative Data for Negative Samples No. Patient U 238 U 235 U238/U235 Sigma 1 G.B. 99.2782 0.7145 139.0 1.3 2 B.B 99.2742 0.7076 140.3 0.2 4 L.B. 99.2738 0.7180 138.3 0.5 5 D.B. 99.2701 0.7233 137.5 0.5 6 P.C. 99.2570 0.7210 137.7 0.5 7 C.C. 99.2738 0.7113 139.6 0.4 12 M.K. 99.2762 0.7152 138.8 0.8 13 C.P.L. 99.2702 0.7200 137.9 0.5 17 C.O. 99.2811 0.7135 139.1 0.9 20 P.R. 99.2742 0.7189 138.1 0.8 Totals 99.2726 0.7166 138.6 0.91 Std. Dev 0.00625 0.0046 0.862 Std. Error 0.00188 0.0014 0.260

Table 5: Ratio of Uranium Isotopes U 238 U 235 U238/U235 U235/U238 Natural Uranium 99.2739 0.7200 137.88 0.0073 Shrapnel (DU) 99.7945 0.2026 492.60 0.0020 Urine 99.3728 0.6119 178.1 0.0062